Confined Fe-Cu Clusters as Sub-Nanometer Reactors for Efficiently Regulating the Electrochemical Nitrogen Reduction Reaction.

atomic clusters electrochemical nitrogen fixation graphitic carbon nitride sub-nanometer reactors synergistic effect

Journal

Advanced materials (Deerfield Beach, Fla.)
ISSN: 1521-4095
Titre abrégé: Adv Mater
Pays: Germany
ID NLM: 9885358

Informations de publication

Date de publication:
Oct 2020
Historique:
received: 28 06 2020
revised: 01 08 2020
pubmed: 3 9 2020
medline: 3 9 2020
entrez: 3 9 2020
Statut: ppublish

Résumé

Electrochemical nitrogen reduction reaction (NRR) over nonprecious-metal and single-atom catalysts has received increasing attention as a sustainable strategy to synthesize ammonia. However, the atomic-scale regulation of such active sites for NRR catalysis remains challenging because of the large distance between them, which significantly weakens their cooperation. Herein, the utilization of regular surface cavities with unique microenvironment on graphitic carbon nitride as "subnano reactors" to precisely confine multiple Fe and Cu atoms for NRR electrocatalysis is reported. The synergy of Fe and Cu atoms in such confined subnano space provides significantly enhanced NRR performance, with nearly doubles ammonia yield and 54%-increased Faradic efficiency up to 34%, comparing with the single-metal counterparts. First principle simulation reveals this synergistic effect originates from the unique Fe-Cu coordination, which effectively modifies the N

Identifiants

DOI: 10.1002/adma.202004382 PMID: 32876982
pubmed: 32876982
doi: 10.1002/adma.202004382
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

e2004382

Subventions

Organisme : National Natural Science Foundation of China
ID : 21905202
Organisme : Guangdong Innovation Research Team for Higher Education
ID : 2017KCXTD030
Organisme : High-level Talents Project of Dongguan University of Technology
ID : KCYKYQD2017017
Organisme : Australian Research Council
ID : DP200100365
Organisme : Discovery Early Career Researcher Award scheme
ID : DE170100871

Informations de copyright

© 2020 The Authors. Published by Wiley-VCH GmbH.

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Auteurs

Xiaowei Wang (X)

Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education, School of Materials Science and Engineering, Tianjin University, Tianjin, 300350, China.
Applied Physics Department, College of Physics and Materials Science, Tianjin Normal University, No. 393 Binshui West Road, Xiqing District, Tianjin, 300387, China.
Institute for Superconducting and Electronic Materials, University of Wollongong, Wollongong, NSW, 2522, Australia.

Siyao Qiu (S)

Science & Technology Innovation Institute, Dongguan University of Technology, Dongguan, 523000, China.

Jianmin Feng (J)

Applied Physics Department, College of Physics and Materials Science, Tianjin Normal University, No. 393 Binshui West Road, Xiqing District, Tianjin, 300387, China.

Yueyu Tong (Y)

Institute for Superconducting and Electronic Materials, University of Wollongong, Wollongong, NSW, 2522, Australia.

Fengling Zhou (F)

Science & Technology Innovation Institute, Dongguan University of Technology, Dongguan, 523000, China.

Qinye Li (Q)

Department of Chemistry and Biotechnology, and Centre for Translational Atomaterials, FSET, Swinburne University of Technology, Hawthorn, Victoria, 3122, Australia.

Li Song (L)

National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui, 230029, China.

Shuangming Chen (S)

National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui, 230029, China.

Kuang-Hsu Wu (KH)

School of Chemical Engineering, The University of New South Wales, Kensington, Sydney, NSW, 2052, Australia.

Panpan Su (P)

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.

Sheng Ye (S)

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.

Feng Hou (F)

Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education, School of Materials Science and Engineering, Tianjin University, Tianjin, 300350, China.

Shi Xue Dou (SX)

Institute for Superconducting and Electronic Materials, University of Wollongong, Wollongong, NSW, 2522, Australia.

Hua Kun Liu (HK)

Institute for Superconducting and Electronic Materials, University of Wollongong, Wollongong, NSW, 2522, Australia.

Gao Qing Max Lu (GQ)

DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering, and Advanced Technology Institute, University of Surrey, Guilford, Surrey, GU2 7XH, UK.

Chenghua Sun (C)

Department of Chemistry and Biotechnology, and Centre for Translational Atomaterials, FSET, Swinburne University of Technology, Hawthorn, Victoria, 3122, Australia.

Jian Liu (J)

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.
DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering, and Advanced Technology Institute, University of Surrey, Guilford, Surrey, GU2 7XH, UK.
ORCID: 0000-0002-5114-0404

Ji Liang (J)

Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education, School of Materials Science and Engineering, Tianjin University, Tianjin, 300350, China.
Institute for Superconducting and Electronic Materials, University of Wollongong, Wollongong, NSW, 2522, Australia.

Classifications MeSH